首页|纳米多级孔SAPO-11分子筛制备及其催化2-甲基萘烷基化反应

纳米多级孔SAPO-11分子筛制备及其催化2-甲基萘烷基化反应

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SAPO-11分子筛作为微孔沸石,通常粒径大,而粒径小的SAPO-11分子筛具有较短的孔道,更有利于分子的扩散使SAPO-11分子筛具有更高的催化活性,但存在稳定性较差的缺点,如何在水热法基础上进一步合成纳米多级孔SAPO-11分子筛极具挑战.在水热合成SAPO-11分子筛基础上,通过对前驱体凝胶进行老化处理制备纳米多级孔SAPO-11分子筛.其中,在80 ℃用搅拌老化制备的SAPO-11分子筛有最小晶体尺寸,通过SEM可知通过搅拌老化制备的Sll-80 ℃-stirring分子筛呈现一种均匀纳米棒状结构,这些纳米棒的直径约500~700 nm,长度约2~4 μm.通过N2吸附-脱附曲线及孔径分布图可知经过老化处理的SAPO-11分子筛较传统SAPO-11都具有更大的比表面积,搅拌老化与静置老化制备的分子筛相比而言具有更大的微孔比表面积与孔体积.且通过NH3-TPD对SAPO-11分子筛酸性性质进行表征,所有老化处理合成的SAPO-11分子筛酸量都有所下降.2-甲基萘(2-MN)主要来源于煤焦油,可用于制备2,6-二甲基萘(2,6-DMN),用于合成高端聚酯,为此将上述纳米多级孔SAPO-11分子筛用于催化2-甲基萘烷基化反应,结果表明使用老化处理制备的纳米多级孔SAPO-11分子筛有77.8%的2-MN初始转化率,20.4%的初始选择性,2,6-DMN、2,7-DMN的物质的量比为1.13,反应第4小时有最高2,6-DMN选择性39.9%,通过系列表征揭示了纳米多级孔SAPO-11分子筛择形催化催化机理.
Preparation of hierarchical nano-SAPO-11 zeolites as catalysts for the synthesis of 2,6-dimethylnaphthalene
As a microporous zeolite,SAPO-11 zeolites usually have a large particle size,and SAPO-11 with a small particle size has shorter pores,which facilitate better diffusion of molecules and thus enhance catalytic activity.However,this also leads to poorer stability.How to further synthesize hierarchical nano-SAPO-11 zeolites on the basis of hydrothermal method is a great challenge.Based on the hy-drothermal method,SAPO-11 zeolites were prepared by aging treatment with the precursor gel.Among them,the SAPO-11 zeolites pre-pared by stirring aging treatment at 80 ℃ has the smallest crystal size.It can be seen by SEM that the S1 1-80 ℃-stirring zeolite show a uniform nanorod-like structure,these nanorods have a diameter of about 500-700 nm and a length of about 2-4 μm.The N2 adsorption-desorption isotherms and pore size distribution curve reveal that the SAPO-11 zeolite treated by aging has a larger specific surface are-a compared to conventional SAPO-11.Specifically,zeolites prepared by agitation aging show a higher specific surface area and pore vol-ume for micropores,but lower values for mesopores compared to those prepared by static aging.The NH3-TPD curves characterization of the acidic properties shows that all SAPO-11 zeolites synthesized with aging treatment have reduced acidity.2-Methylnaphthalene(2-MN),which is mainly derived from coal tar,can be used to prepare 2,6-dimethylnaphthalene(2,6-DMN),and then be used to synthesize high-end polyester.Therefore,the above-mentioned hierarchical nano-SAPO-11 zeolites were applied to catalyze the alkyla-tion reaction of 2-methylnaphthalene.The results show that the SAPO-11 zeolites prepared by aging treatment have 77.8%initial conver-sion of 2-MN,20.4%initial selectivity,1.13 molar ratio of 2,6-DMN/2,7-DMN,and the highest selectivity of 2,6-DMN of 39.9%at the 4th hour of reaction.The shape selection catalytic mechanism of SAPO-11 molecular sieve was revealed by series characterization.

hierarchical poreSAPO-11aging treatmentalkylation2,6-dimethylnaphthalene

张晓华、张璞、纪琳、江乐杰、宋艳萍、魏海国、曾庆峰、叶闰平、冯刚

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中国石油天然气股份有限公司规划总院,北京 100083

中国石油炼油化工和新材料分公司,北京 100007

辽河油田油气集输公司,辽宁盘锦 124010

南昌大学化学化工学院,江西南昌 330031

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多级孔 SAPO-11 老化处理 烷基化 2,6-二甲基萘

国家自然科学基金资助项目国家自然科学基金资助项目江西省双高资助项目

2236202221875096

2024

洁净煤技术
煤炭科学研究总院 煤炭工业洁净煤工程技术研究中心

洁净煤技术

CSTPCD北大核心
影响因子:0.893
ISSN:1006-6772
年,卷(期):2024.30(8)